Spectral Properties of delta-Plutonium: Sensitivity to 5f Occupancy

Abstract

By combining the local density approximation (LDA) with dynamical mean field theory (DMFT), we report a systematic analysis of the spectral properties of $\delta$-plutonium with varying $5f$ occupancy. The LDA Hamiltonian is extracted from a tight-binding (TB) fit to full-potential linearized augmented plane-wave (FP-LAPW) calculations. The DMFT equations are solved by the exact quantum Monte Carlo (QMC) method and the Hubbard-I approximation. We have shown for the first time the strong sensitivity of the spectral properties to the $5f$ occupancy, which suggests using this occupancy as a fitting parameter in addition to the Hubbard $U$. By comparing with PES data, we conclude that the ``open shell'' $5f^5$ configuration gives the best agreement, resolving the controversy over $5f$ ``open shell'' versus ``close shell'' atomic configurations in $\delta$-Pu.

6 pages, 2 embedded color figures, to appear in Physical Review B

References in corpus (5)

• What is the valence of a correlated solid? The double life of delta-plutonium
• Magnetic state of plutonium ion in metallic Pu and its compounds
• Thermodynamic and spectral properties of compressed Ce calculated by the merger of the local density approximation and dynamical mean field theory
• Electronic structure and non-magnetic character of $\delta$-Pu-Am alloys
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Cited by in corpus (7)

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• Many-body Electronic Structure of Metallic alpha-Uranium
• Electronic structure and spectral properties of Am, Cm and Bk: Charge density self-consistent LDA+HIA calculations in FP-LAPW basis
• X-ray absorption branching ratio in actinides: LDA+DMFT approach
• Does hybrid density functional theory predict a non-magnetic ground state for delta-Plutonium?
• Exchange energy dominated by large orbital spin-currents in $\delta$-Pu
• Coulomb correlation in presence of spin-orbit coupling: application to plutonium